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Register a new userOptically induced spin polarisation of the NV- centre in diamond: role of electron-vibration interaction
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The novel aspect of the centre (NV-) in diamond is the high degree of spin polarisation achieved through optical illumination. In this paper it is shown that the spin polarisation occurs as a consequence of an electron-vibration interaction combined with spin-orbit interaction, and an electronic model involving these interactions is developed to account for the observed polarisation.
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The characteristic transition of the NV- centre at 637 nm is between ${}^3mathrm{A}_2$ and ${}^3mathrm{E}$ triplet states. There are also intermediate ${}^1mathrm{A}_1$ and ${}^1mathrm{E}$ singlet states, and the infrared transition at 1042 nm between these singlets is studied here using uniaxial stress. The stress shift and splitting parameters are determined, and the physical interaction giving rise to the parameters is considered within the accepted electronic model of the centre. It is established that this interaction for the infrared transition is due to a modification of electron-electron Coulomb repulsion interaction. This is in contrast to the visible 637 nm transition where shifts and splittings arise from modification to the one-electron Coulomb interaction. It is also established that a dynamic Jahn-Teller interaction is associated with the singlet ${}^1mathrm{E}$ state, which gives rise to a vibronic level 115 $mathrm{cm}^{-1}$ above the ${}^1mathrm{E}$ electronic state. Arguments associated with this level are used to provide experimental confirmation that the ${}^1mathrm{A}_1$ is the upper singlet level and ${}^1mathrm{E}$ is the lower singlet level.
The study establishes that the degree of optically induced spin polarization that can be achieved for NV$^- $in 1b diamond is limited by the concentration of single substitutional nitrogen, N$^0$ . The polarization of the individual NV centres in the diamond is dependent on the separation of the NV$^-$ and the nitrogen donor. When the NV$^-$ - N$^+$ pair separation is large the properties of the pair will be as for single sites and a high degree of spin polarization attainable. When the separation decreases the emission is reduced, the lifetime shortened and the spin polarization downgraded. The deterioration occurs as a consequence of electron tunneling in the excited state from NV$^-$ to N$^+$ and results in an optical cycle that includes NV$^0$. The tunneling process is linear in optical excitation and more prevalent the closer the N$^+$ is to the NV$^-$ centre. However, the separation between the NV$^-$ and its donor N$^+$ can be effected by light through the excitation of NV$^-$ and/or ionization of N$^0$. The optical excitation that creates the spin polarization can also modify the sample properties and during excitation creates charge dynamics. The consequence is that the magnitude of spin polarization, the spin relaxation and coherence times T$_1$ and T$_2$ have a dependence on the nitrogen concentration and on the excitation wavelength. The adjacent N$^+$ gives an electric field that Stark shifts the NV$^-$ transitions and for an ensemble results in line broadening. It is observation of changes of these Stark induced effects that allow the variation in NV$^-$ - N$^+$ separation to be monitored. Spectroscopic measurements including that of the varying line widths are central to the study. They are made at low temperatures and include extensive measurements of the NV$^-$ optical transition at 637 nm, the infrared transition at 1042 nm and ODMR at 2.87 GHz.
The sensitivity of Magnetic Resonance Imaging (MRI) depends strongly on nuclear spin polarisation and, motivated by this observation, dynamical nuclear spin polarisation has recently been applied to enhance MRI protocols (Kurhanewicz, J., et al., Neoplasia 13, 81 (2011)). Nuclear spins associated with the 13 C carbon isotope (nuclear spin I = 1/2) in diamond possess uniquely long spin lattice relaxation times (Reynhardt, E.C. and G.L. High, Prog. in Nuc. Mag. Res. Sp. 38, 37 (2011)) If they are present in diamond nanocrystals, especially when strongly polarised, they form a promising contrast agent for MRI. Current schemes for achieving nuclear polarisation, however, require cryogenic temperatures. Here we demonstrate an efficient scheme that realises optically induced 13 C nuclear spin hyperpolarisation in diamond at room temperature and low ambient magnetic field. Optical pumping of a Nitrogen-Vacancy (NV) centre creates a continuously renewable electron spin polarisation which can be transferred to surrounding 13 C nuclear spins. Importantly for future applications we also realise polarisation protocols that are robust against an unknown misalignment between magnetic field and crystal axis.
Using pulsed photoionization the coherent spin manipulation and echo formation of ensembles of NV- centers in diamond are detected electrically realizing contrasts of up to 17 %. The underlying spin-dependent ionization dynamics are investigated experimentally and compared to Monte-Carlo simulations. This allows the identification of the conditions optimizing contrast and sensitivity which compare favorably with respect to optical detection.
We propose a high efficiency high fidelity measurement of the ground state spin of a single NV center in diamond, using the effects of cavity quantum electrodynamics. The scheme we propose is based in the one dimensional atom or Purcell regime, removing the need for high Q cavities that are challenging to fabricate. The ground state of the NV center consists of three spin levels $^{3}A_{(m=0)}$ and $^{3}A_{(m=pm1)}$ (the $pm1$ states are near degenerate in zero field). These two states can undergo transitions to the excited ($^{3}E$) state, with an energy difference of $approx7-10$ $mu$eV between the two. By choosing the correct Q factor, this small detuning between the two transitions results in a dramatic change in the intensity of reflected light. We show the change in reflected intensity can allow us to read out the ground state spin using a low intensity laser with an error rate of $approx5.5times10^{-3}$, when realistic cavity and experimental parameters are considered. Since very low levels of light are used to probe the state of the spin we limit the number of florescence cycles, thereby limiting the non spin preserving transitions through the intermediate singlet state $^{1}A$.
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